JP2016141611A - Composition for joint - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a composition for joint high in joint strength when joining a material to be jointed containing a metal or oxide or the like in a joint part.SOLUTION: There is provided a composition for joint containing tin as a main component, silver of 0.5 to 11.0 mass% and iridium, where the content of tin is preferably 60% or more, further preferably 84% or more, especially preferably 92 mass% or more. There is provided a composition for joint further containing, by mass%, 0.001≤Ir≤1.0%, 0.001≤Al≤0.8%, 0≤Ge≤1.0%, 0≤Ni≤1.0%, 0≤Cu≤0.1%, 0≤Mg≤0.5% and 0.0001≤O≤2.SELECTED DRAWING: None

Description

  The present invention relates to a bonding composition.

  Conventionally, a bonding composition that can be used when bonding a material to be bonded that includes a metal, an oxide, or the like in a bonding portion has been studied. In particular, since it is difficult to bond a material to be bonded containing an oxide to the bonding portion, a bonding composition that can be bonded even when an oxide is included in the bonding portion of the material to be bonded has been studied. ing.

  For example, Patent Document 1 includes, in mass%, Ag: 2.0 to 15.0%, Al: more than 0.1 to 6.0%, and the remaining Sn and inevitable impurities. A solder alloy for joining objects is disclosed.

Patent No. 46669877

  However, in recent years, there has been a demand for a bonding composition that exhibits higher bonding strength when bonding materials to be bonded. For this reason, even the solder alloy for oxide bonding disclosed in Patent Document 1 has a problem that the bonding strength is not sufficient.

  In view of the problems of the above-described conventional technology, an object of the present invention is to provide a bonding composition having high bonding strength.

In one embodiment of the present invention to solve the above problems, tin, silver, and iridium are contained,
Containing tin as a main component,
A bonding composition containing 0.5% by mass or more and 11.0% by mass or less of the silver is provided.

  According to one embodiment of the present invention, a bonding composition having high bonding strength can be provided.

In an Example and a comparative example, the schematic explanatory drawing of the 3 point | piece bending test for evaluating joining strength. Explanatory drawing of the preparation procedure of the test piece for a three-point bending test. The schematic explanatory drawing of the leak test which evaluates the vacuum sealing characteristic of a joint surface in an Example and a comparative example.

  DESCRIPTION OF EMBODIMENTS Hereinafter, embodiments for carrying out the present invention will be described with reference to the drawings. However, the present invention is not limited to the following embodiments, and the following embodiments are not departed from the scope of the present invention. Various modifications and substitutions can be made.

  In this embodiment, first, one structural example of the bonding composition will be described.

  The bonding composition of the present embodiment contains tin, silver, and iridium, contains tin as a main component, and contains 0.5% by mass or more and 11.0% by mass or less of silver.

Below, each component which the composition for joining of this embodiment can contain is demonstrated.
(Tin)
As described above, the bonding composition of this embodiment contains tin (Sn) as a main component. Tin can relieve the difference in thermal expansion between the material to be joined and the composition for joining. Furthermore, tin has a function of lowering the melting temperature of the bonding composition.

  The phrase “contained as a main component in the bonding composition” means, for example, the component that is contained most in the bonding composition, and is 60% by mass in the bonding composition. It is preferable that it is the component contained above.

  In particular, the content of tin in the bonding composition is, for example, more preferably 84% by mass or more, and further preferably 92% by mass or more.

  In the case where the tin content in the bonding composition is 84% by mass or more, the relaxation of the difference in thermal expansion between the above-described bonded material and the bonding composition and the decrease in the melting temperature of the bonding composition This is because a particularly high effect is exhibited.

  The upper limit of the content of tin in the bonding composition is not particularly limited, but is preferably 99% by mass or less, and more preferably 98% by mass or less.

As described above, the bonding composition of the present embodiment contains silver and iridium in addition to tin. And by containing these components, the joining strength of a to-be-joined material can be raised especially. In addition to silver and iridium, optional components described later can be added. For this reason, in order to fully ensure content of components other than these tin, as above-mentioned, it is preferable that content of tin is 99 mass% or less.
(Silver)
As described above, the bonding composition of this embodiment contains silver.

  When the bonding composition contains silver, high bonding strength can be exhibited even when an oxide is contained in the bonded portion of the material to be bonded.

  This is because silver can be combined with oxygen, and by containing silver, it is possible to improve the bondability with an oxide contained in the bonded portion of the material to be bonded and the wettability.

  Note that when the bonding composition forms an oxide film combined with oxygen, the bonding with the material to be bonded may be hindered. However, the silver combined with oxygen does not form an oxide film but is mainly bonded. It is thought that it is contained in the composition for use. And it can also suppress that an oxide film arises in the composition for joining itself because the composition for joining contains silver.

  Moreover, although the composition for joining of this embodiment can contain tin as a main component as mentioned above, since tin is a comparatively soft metal, sufficient joining strength cannot be obtained only with tin. On the other hand, the bonding composition of the present embodiment contains tin and silver at the same time, so that tin and silver can form an intermetallic compound, thereby increasing the bonding strength of the bonding composition. become.

  The silver content in the bonding composition of this embodiment is 0.5% by mass or more. The content of silver in the bonding composition of the present embodiment is preferably 1.0% by mass or more, and more preferably 1.5% by mass or more.

  When the silver content in the bonding composition is 0.5% by mass or more, tin and silver form a sufficient amount of intermetallic compound as described above, and the bonding strength of the bonding composition is increased. This is because it can be increased.

  Moreover, the upper limit of content of silver in the composition for joining of this embodiment is 11.0 mass% or less. The upper limit of the silver content in the bonding composition of the present embodiment is preferably 10.0% by mass or less, and more preferably 8.5% by mass or less.

As described above, tin and silver can form an intermetallic compound, but the intermetallic compound of tin and silver is hard, but has brittle characteristics, and the content of such intermetallic compound If the amount increases too much, the bonding strength may decrease. For this reason, it is because it is preferable to make content of silver into 11.0 mass% or less so that the intermetallic compound may not increase more than necessary in the joining composition.
(iridium)
As described above, the bonding composition of the present embodiment contains iridium.

  The inventors of the present invention diligently studied the composition of the bonding composition that can further increase the bonding strength when the materials to be bonded are bonded. And it discovered that airtightness and joining strength could be improved by containing iridium (Ir) which was not used as a constituent material of the composition for joining until now.

  Further, according to the study of the inventors of the present invention, the bonding composition contains iridium, so that the generation of voids is reduced when the bonding composition is melted in order to bond the materials to be bonded together. It also has an effect that can be achieved. This is because, by adding iridium to the bonding composition, the surface tension of the molten metal obtained by melting the bonding composition can be reduced, and the entrainment of gas can be reduced, and the crystal grains of the alloy contained in the bonding composition This is thought to be due to the fact that it can be made finer.

  When voids are generated when the bonding composition is melted, the bonding area is reduced, but according to the bonding composition of the present embodiment containing iridium, the occurrence of voids can be suppressed. It can reduce, and airtightness can be improved. Furthermore, a sufficient bonding area can be secured and the bonding strength can be increased.

  Depending on the content of the conventional bonding composition, when the bonding composition is melted and the materials to be bonded are bonded, an oxide film, which is an oxide film, is generated on the surface of the bonding composition. was there. As described above, once an oxide film is generated on the surface of the bonding composition, it becomes difficult to spread the bonding composition or bond to the material to be bonded. Therefore, when a bonding composition is melted, applied, and bonded to a material to be bonded, an ultrasonic soldering iron that can be heated while applying ultrasonic vibration has been used to destroy the oxide film. .

  On the other hand, according to the bonding composition containing iridium of the present embodiment, it is possible to suppress the generation of an oxide film on the surface when the bonding composition is melted. For this reason, it becomes possible to spread the joining composition or to join the material to be joined using a soldering iron having only a heating function instead of the above-described ultrasonic soldering iron. Alternatively, when the joining composition and the material to be joined are heated in a contact state, the joining composition spreads out without using a soldering iron and can be joined to the material to be joined. Accordingly, restrictions on a processing apparatus such as a soldering iron when the bonding composition is melted and applied to the material to be bonded are reduced, and workability can be improved.

  The iridium content of the bonding composition of the present embodiment is not particularly limited, and can be, for example, 0.001% by mass or more. The content of iridium in the bonding composition of the present embodiment is preferably 0.005% by mass or more, and more preferably 0.008% by mass or more.

  This is because when the content of iridium is 0.001% by mass or more, the bonding strength can be sufficiently increased when the materials to be bonded are bonded by the bonding composition. Moreover, it is because it becomes possible to suppress especially generation | occurrence | production of a void and generation | occurrence | production of an oxide film, when melt | dissolving a joining composition and joining a to-be-joined material.

  The upper limit of the iridium content of the bonding composition of the present embodiment is not particularly limited, but may be, for example, 1.0% by mass or less. The upper limit of the iridium content of the bonding composition of the present embodiment is preferably 0.8% by mass or less, and more preferably 0.5% by mass or less.

  This is because if the iridium content exceeds 1.0 mass%, the melting point of the bonding composition may increase.

  Further, according to the study by the inventors of the present invention, when the iridium content is 1.0% by mass or less, as described above, when the bonding composition is melted, an oxide film is generated on the surface thereof. It is because it can suppress more reliably.

So far, tin, silver, and iridium included in the bonding composition of the present embodiment have been described. However, the bonding composition of the present embodiment may further include an arbitrary component. The optional components are described below.
(aluminum)
The bonding composition of the present embodiment can further contain aluminum (Al).

  When the bonding composition is dissolved, aluminum contained in the bonding composition tends to be an oxide. For this reason, when an oxide is included in the bonding portion of the material to be bonded, the oxide in the bonding portion and the bonding composition are easily bonded, and the bonding composition and the bonding including the oxide This is because the wettability with the part is improved and high bonding strength can be exhibited.

  The aluminum content of the bonding composition of the present embodiment is not particularly limited, and can be, for example, 0.001% by mass or more. The aluminum content of the bonding composition of the present embodiment is preferably 0.01% by mass or more, more preferably 0.03% by mass or more.

  This is because, when the aluminum content of the bonding composition is 0.001% by mass or more, the wettability between the oxide contained in the bonded portion of the material to be bonded and the bonding composition is particularly improved, and the bonding strength is increased. This is because it can be increased.

  Moreover, the upper limit of the aluminum content of the bonding composition of the present embodiment is not particularly limited, but may be, for example, 0.8% by mass or less. The upper limit of the aluminum content of the bonding composition of the present embodiment is preferably 0.5% by mass or less, and more preferably 0.3% by mass or less.

  This is because, as described above, aluminum tends to form an oxide when the bonding composition is melted, but when the aluminum content exceeds 0.8% by mass, the bonding composition is melted. This is because an oxide may be excessively formed in the bonding composition.

  If an oxide is excessively generated in the bonding composition, for example, the oxide may be deposited on the surface of the bonding composition to form an oxide film. If an oxide film is formed on the surface of the bonding composition, the bonding strength with the material to be bonded decreases, or the entire bonding composition becomes porous due to solidification shrinkage, and the airtightness of the bonded portion of the material to be bonded decreases. There is a risk of doing.

  In addition, when the materials to be joined are melted and joined, aluminum may be separated from the joining composition to form an aluminum layer. However, when the aluminum content of the bonding composition is 0.8% by mass or less, even if an aluminum layer is formed, the bonding strength is hardly affected. For this reason, it is preferable that content of aluminum is 0.8 mass% or less.

  Note that the bonding composition of the present embodiment may contain germanium and aluminum described later at the same time. When both are contained simultaneously, it is preferable that it is 1.8 mass% or less in total.

Further, the bonding composition of the present embodiment contains one or more metals selected from germanium (Ge), nickel (Ni), copper (Cu), and magnesium (Mg) as other optional components. You can also. Each component will be described below.
(germanium)
As described above, the bonding composition of the present embodiment can further contain germanium.

  When the bonding composition is dissolved, germanium contained in the bonding composition tends to be an oxide. For this reason, when an oxide is included in the bonding portion of the material to be bonded, the oxide in the bonding portion and the bonding composition are easily bonded, and the bonding composition and the bonding including the oxide This is because the wettability with the part is improved and high bonding strength can be exhibited.

  The germanium content of the bonding composition of the present embodiment is not particularly limited, and can be, for example, 0 mass or more. The germanium content of the bonding composition of the present embodiment is preferably 0.01% by mass or more.

  Moreover, the upper limit value of the germanium content of the bonding composition of the present embodiment is not particularly limited, but may be, for example, 1.0% by mass or less. The upper limit of the germanium content of the bonding composition of the present embodiment is preferably 0.8% by mass or less, and more preferably 0.6% by mass or less.

This is because if the content of germanium exceeds 1.0% by mass, an oxide may be excessively generated in the bonding composition when the bonding composition is melted. This is because, if an oxide is excessively generated in the bonding composition, for example, the oxide is deposited on the surface of the bonding composition to form an oxide film, which may hinder the bonding with the object to be bonded. .
(nickel)
As described above, the bonding composition of the present embodiment can contain nickel (Ni).

  When the bonding composition is dissolved, nickel contained in the bonding composition tends to be an oxide. For this reason, when an oxide is included in the bonding portion of the material to be bonded, the oxide in the bonding portion and the bonding composition are easily bonded, and the bonding composition and the bonding including the oxide This is because the wettability with the part is improved and high bonding strength can be exhibited.

  The nickel content of the bonding composition of the present embodiment is not particularly limited, but can be, for example, 1.0% by mass or less, and preferably 0.5% by mass or less.

  In this case, when the materials to be joined are melted and joined, the nickel may be separated from the joining composition to form a nickel layer. However, when the nickel content is 1.0% by mass or less, even if the nickel layer is formed, there is almost no influence on the bonding strength. For this reason, it is preferable that nickel content is the range of 1.0 mass% or less.

The lower limit of the nickel content of the bonding composition of the present embodiment is not particularly limited, and can be, for example, 0% by mass or more.
(copper)
As described above, the bonding composition of the present embodiment can contain copper (Cu).

  When the bonding composition contains copper, the melting point of the bonding composition can be lowered. Moreover, it is because it becomes possible to improve the wettability with respect to the to-be-joined material of a joining composition, and to exhibit high joining strength because the joining composition contains copper.

  Although content of copper of the composition for joining of this embodiment is not specifically limited, For example, it can be 0.1 mass% or less.

  This is because copper has a function of lowering the melting point of the bonding composition as described above. However, if the copper content is excessively increased, the melting point of the bonding composition may be increased. Then, it can prevent more reliably that melting | fusing point of the composition for joining goes up by making content of copper into 0.1 mass% or less.

The lower limit of the copper content of the bonding composition of the present embodiment is not particularly limited, and can be, for example, 0% by mass or more.
(magnesium)
As described above, the bonding composition of the present embodiment can contain magnesium (Mg).

  When the bonding composition is dissolved, magnesium contained in the bonding composition tends to be an oxide. For this reason, when an oxide is included in the bonding portion of the material to be bonded, the oxide in the bonding portion and the bonding composition are easily bonded, and the bonding composition and the bonding including the oxide This is because the wettability with the part is improved and high bonding strength can be exhibited.

  The magnesium content of the bonding composition of the present embodiment is not particularly limited, but can be, for example, 0.5% by mass or less, and preferably 0.3% by mass or less.

  This is because magnesium is a metal that is easily corroded, and if the magnesium content is too high, the bonding composition itself may become brittle. By making the magnesium content 0.5% by mass or less, it is possible to more reliably suppress the occurrence of corrosion.

  The lower limit of the magnesium content of the bonding composition of the present embodiment is not particularly limited, and can be, for example, 0% by mass or more.

  So far, although each component which the composition for joining of this embodiment can contain was demonstrated, it is not limited to the material which concerns. Moreover, the bonding composition of the present embodiment may contain inevitable components that are generated, for example, when preparing the bonding composition. The inevitable component is not particularly limited. However, when one or more elements selected from Fe, Co, Cr, V, Mn, Sb, Pb, Bi, Zn, As, and Cd are contained as unavoidable components, the content of the above elements is 0 in total. It is preferably 2% by mass or less, and more preferably 0.05% by mass or less in total.

  This is because the element has a function of reducing the wettability of the bonding composition to the material to be bonded, and the total content of the elements is 0.2% by mass or less. It is because it can suppress that the wettability with respect to a material falls.

  Moreover, since Ga, P, and B cause the generation of voids, when one or more elements selected from Ga, P, and B are contained as inevitable components, the total content is 0.05% by mass or less. It is preferable that it is 0.01 mass% or less in total.

  And the composition for joining of this embodiment can contain oxygen further.

  Oxygen in the bonding composition is a component that promotes bonding between the bonding composition and the bonding portion containing the oxide when the bonding portion of the material to be bonded contains an oxide.

  Although the state of oxygen contained in the bonding composition is not particularly limited, for example, oxygen is preferably contained in a dissolved form in the metal material. This is because the oxygen concentration gradient between the oxide of the bonded portion of the material to be bonded and the metal in the bonding composition becomes smooth at the interface between the bonding composition and the material to be bonded. This is because it becomes stronger.

  The method for containing oxygen in the bonding composition is not particularly limited. For example, a method for dissolving and manufacturing the bonding composition in an atmosphere containing oxygen, or a material to be joined in an atmosphere containing oxygen. And a method of performing the joining work.

  In addition, it is preferable that the bonding composition before bonding the material to be bonded satisfies the oxygen content in the bonding composition. For this reason, it is preferable to adjust oxygen concentration by the method of melt | dissolving and manufacturing the joining composition in the atmosphere containing oxygen.

  In particular, it is more preferable that the oxygen content satisfies the above range in any state of the bonding composition before bonding the materials to be bonded and the bonding composition after bonding.

  The oxygen content in the bonding composition is not particularly limited, but may be, for example, 0.0001% by mass or more, and preferably 0.0007% by mass or more.

  This is because the effect of increasing the bonding strength can be sufficiently exhibited by setting the oxygen content to 0.0001 mass% or more.

  The upper limit of the content of oxygen in the bonding composition is not particularly limited, but may be, for example, 2% by mass or less, and preferably 1% by mass or less.

  This is because if the amount of oxygen contained in the bonding composition is excessively large, oxides are likely to be deposited on the surface of the metal material or inside thereof, and the bonding strength may be lowered. For this reason, as described above, the oxygen content in the bonding composition is preferably 2% by mass or less.

  Here, the oxygen content in the bonding composition herein means the content of oxygen contained in the bonding composition. That is, when the oxide film is formed on the bonding composition surface, the oxygen content in the bonding composition after the oxide film is removed is shown.

  When measuring the amount of oxygen in the bonding composition, the method for removing the oxide film is not particularly limited, and for example, it can be removed by treating the surface of the bonding composition with an acid or the like.

  Up to this point, the bonding composition of the present embodiment has been described. However, the material to be bonded by the bonding composition of the present embodiment is not particularly limited, and may be used for bonding various types of bonded materials. it can. Examples of the material to be joined include metals and oxides, and can be used for joining metals, joining oxides, and joining metals and oxides.

  In particular, in the past, when an oxide was included in the joint portion of the material to be joined, it was difficult to provide sufficient joint strength. However, according to the joining composition of this embodiment, high joint strength is exhibited. be able to. For this reason, the bonding composition of the present embodiment can be particularly suitably used when bonding a material to be bonded containing an oxide at a bonding portion.

  In addition, although the oxide contained in the junction part of a to-be-joined material is not specifically limited, For example, it is preferable that it is 1 or more types selected from glass, chromium oxide, and aluminum oxide. The chromium oxide includes chromium oxide formed on the surface of stainless steel. Further, the aluminum oxide includes a passive film formed on the surface of aluminum metal and aluminum oxide.

  Specific examples will be described below, but the present invention is not limited to these examples.

First, the evaluation method of the composition for joining manufactured in the following example and the comparative example is demonstrated.
(Joint strength)
Test pieces were prepared by connecting two glass plates with the bonding compositions prepared in the following examples and comparative examples. The test pieces were tested by three-point bending, and the bonding strength (unit: N / mm). ² ) was measured.

  A specific test procedure will be described with reference to FIGS. FIG. 1 schematically shows a cross-sectional view of a test piece in a plane parallel to the laminating direction of two glass plates constituting the test piece. FIG. 2 is an explanatory diagram for the procedure for producing the test piece shown in FIG. The same numbers are attached to the same members in FIGS.

  As shown in FIG. 1, in the three-point bending test, a joining composition constituted by a joining composition at a bonding margin of 5 mm in length at a position where two soda lime glass substrates 111 and 112 are displaced from each other. The test piece joined by the part 12 was used. Then, the bottom surface of the joined test piece is supported by support jigs 131 and 132, and the load is applied in the direction of the block arrow A through the jig 14 on the upper surface side of the joined test piece while suppressing the bonding margin. Was added to perform a three-point bending test.

  In the three-point bending test, the load was measured when the joint was peeled off and separated into two glass plates, or the test piece was broken. And the measured value was made into joint strength of the used composition for joining.

  Model 1308 manufactured by Aiko Engineering Co., Ltd. was used as the load evaluation tester.

  Here, a procedure for producing the test piece shown in FIG. 1 will be described with reference to FIG.

  As shown in FIG. 2A, two soda lime glass substrates 111 and 112 each having a thickness of 5 mm, a length of 30 mm, and a width of 30 mm were prepared. Then, the bonding compositions prepared in the examples and comparative examples are heated to 300 ° C. by the soldering iron 22 on the bonding margin (length 5 mm × width 30 mm) provided along one side of the soda-lime glass substrates 111 and 112. To form bonding composition portions 211 and 212.

  After that, the soda-lime glass substrates 111 and 112 and the applied bonding composition are cooled, so that the bonding composition does not flow, specifically even when the front and back of the soda-lime glass substrates 111 and 112 are reversed. The composition was solidified to such an extent that it did not flow. At this time, the bonding composition was cooled to 160 ° C. or lower.

  Next, as shown in FIG. 2 (B), the front and back surfaces of the soda lime glass substrate 111 are reversed, and applied and formed on the bonding margins of the soda lime glass substrates 111 and 112. Was brought into contact. In this state, the soda lime glass substrates 111 and 112 were heated to 300 ° C.

  After the heating, the soda lime glass substrate and the bonding composition were cooled, and the bonding composition was solidified to obtain the test piece shown in FIG.

Note that the bonding composition portions 211 and 212 applied and formed on the soda lime glass substrates even when the bonding composition portions 211 and 212 applied and formed on the margins of the soda lime glass substrates 111 and 112 are brought into contact with each other and heated. Some specimens 212 did not integrate. This is because very thin oxide films are formed on the surfaces of the bonding composition portions 211 and 212. In Examples and Comparative Examples 1 and 3, as shown in FIG. 2 (C), the soldering iron 23 is applied lightly to the soda lime glass substrates 111 and 112 so as to be inserted between the formed composition parts. It was possible to easily destroy the oxide film formed on the surfaces of the bonding composition portions 211 and 212 and to make the bonding composition portion 12 integrated. However, in Comparative Examples 2, 4 and 5, the bonding composition portions 211 and 212 applied and formed on the bonding margin of the soda lime glass substrates 111 and 112 are contacted, heated, and a soldering iron is contacted. The bonding composition portions 211 and 212 applied and formed on each soda lime glass substrate were not bonded and were not integrated. This is presumably because a strong oxide film was formed on the surfaces of the bonding composition portions 211 and 212, which could not be destroyed by a soldering iron having only a heating function without an ultrasonic impact function.
(Airtightness test)
A method of the airtightness test will be described with reference to FIG. FIG. 3 shows a perspective view of a test piece of the airtightness test.

  Soda lime glass substrates 31 and 33 having a thickness of 5 mm × length of 50 mm × 50 mm were prepared. One soda-lime glass substrate 33 had a 3 mmφ hole 331 formed in the center in advance. Then, the soda-lime glass substrates 31 and 33 are bonded to the soda-lime glass substrates using the bonding compositions prepared in the respective examples and comparative examples so as to have a width of about 2 mm around one plane, that is, along the four sides. It heated with the soldering iron so that it might become 300 degreeC above, and it applied.

  The soda lime glass substrate and the applied bonding composition are cooled to such an extent that the bonding composition does not flow, specifically, even when the front and back of the soda lime glass substrates 31 and 33 are reversed. It solidified to such an extent that it did not flow. At this time, the bonding composition was cooled to 160 ° C. or lower.

  Next, the soda-lime glass substrates 31 and 33 were overlapped so that the surfaces to which the bonding composition was applied face each other. Under the present circumstances, it arrange | positions so that the composition for joining apply | coated to each soda-lime glass substrate may contact. The soda lime glass substrates 31 and 33 were heated to 300 ° C. and bonded. Thereafter, it was cooled to obtain a test piece.

  Since a 0.35 mm thick stainless steel piece is installed as a spacer between the soda lime glass substrate 31 and the soda lime glass substrate 33, a container having a height space of 0.35 mm inside It has become.

  In addition, for test specimens where the joining composition applied to each soda lime glass substrate does not integrate even when the soda lime glass substrates are overlaid and heated, lightly so that the soldering iron is inserted between the joining compositions. It was possible to integrate by contacting. However, in Comparative Examples 2, 4 and 5, when soda lime glass substrates are overlaid and the bonding compositions are bonded to each other, bonding is performed in the same manner as in the three-point bending test even if the soldering iron is brought into contact. I could not.

  And with respect to the obtained container, the amount of leaks was measured using a leak detector (HELIOT 700 manufactured by ULVAC, Inc.) while vacuum degassing the space and blowing He gas to each part of the joint.

When the measured leak amount was 1.0 × 10 ⁻¹¹ (Pa · m ³ / s) or less, it was determined to be acceptable. Moreover, when the measured leak amount ^exceeded 1.0 * 10 < ^-11 > (Pa * m < ³ > / s), it determined with disqualification. In Table 1, “OK” indicates “good”, and “X” indicates failure.
(Measurement of oxygen content in bonding composition)
The oxygen content contained in the bonding composition of Example 25 shown in Table 2 was measured by the following procedures (1) to (3).
(1) As a sample for analysis, 0.5 g of a small piece of the produced bonding composition was prepared.
(2) Chemical etching was performed to remove the influence of the oxide film contained on the surface of the small piece of the bonding composition prepared in (1).

Specifically, a beaker containing a small piece of the bonding composition and 2-fold diluted hydrochloric acid was set in a water bath and heated at 80 ° C. for 12 minutes. Thereafter, decantation was performed with degassed water, followed by decantation with ethanol.
(3) The oxygen concentration of the sample of the bonding composition from which the oxide film was removed in (2) was measured. The measurement was performed using an oxygen / hydrogen analyzer (LECO Corporation model: ROH-600).

Below, the composition for joining of each Example and a comparative example is demonstrated.
[Example 1]
Sn, Ag, and Ir were weighed, mixed and dissolved so that each component contained in the bonding composition had the composition shown in Table 1, and then poured into a mold to prepare a bonding composition.

  And about the produced joining composition, the above-mentioned joining strength test and an airtight test were implemented. The results are shown in Table 1.

In Table 1, the content of Sn is described as “Remainder”, but this is the content of Sn after subtracting the content of components other than Sn shown in Table 1 from 100% by mass. It shows that. The same applies to Examples and Comparative Examples other than Example 1.
[Examples 2 to 25]
Similar to Example 1 except that Sn, Ag, Ir, and each component shown in Table 1 were weighed and mixed so that each composition had the composition shown in Table 1 when the bonding composition was prepared. Thus, a bonding composition was prepared and evaluated. For Example 25, the oxygen content in the bonding composition was also measured.

The evaluation results are shown in Table 1.
[Comparative Examples 1 to 5]
When the bonding composition was prepared, the bonding composition was prepared and evaluated in the same manner as in Example 1 except that each component was weighed and mixed so that each composition had the composition shown in Table 1. went.

  The results are shown in Table 1.

表１に示した結果によると、Ｓｎ、Ａｇ、Ｉｒを含有し、かつＳｎを主成分として含有し、Ａｇの含有量が０．５質量％以上１１．０質量％以下となっている実施例１〜実施例２５は、Ａｇの含有量が０．５質量％未満若しくは１１質量％より大きい、またはＩｒを含まない、比較例１〜比較例５に対して高い接合強度を示すことが確認できた。特に比較例２、４および５においては、接合用組成物表面に強固な酸化皮膜が形成されていた。このため、上述のように試験片を作製する際に超音波衝撃機能を持たない加熱機能のみのはんだごてを用い、表面に形成された酸化皮膜の破壊を試みたが、接合することさえできず、サンプルの作製ができなかった。

According to the results shown in Table 1, Examples containing Sn, Ag, Ir, containing Sn as a main component, and the Ag content being 0.5 mass% or more and 11.0 mass% or less. It can be confirmed that Examples 1 to 25 show a high bonding strength with respect to Comparative Examples 1 to 5 in which the Ag content is less than 0.5% by mass or more than 11% by mass or does not contain Ir. It was. Particularly in Comparative Examples 2, 4 and 5, a strong oxide film was formed on the surface of the bonding composition. For this reason, when preparing a test piece as described above, an attempt was made to destroy the oxide film formed on the surface using only a heating iron that does not have an ultrasonic impact function, but it could even be joined. The sample could not be prepared.

  From the comparison of the bonding strength of the bonding compositions of Examples 1 to 25 and the bonding strength of the bonding compositions of Comparative Examples 1 to 5, in the bonding compositions of Examples 1 to 25 Confirmed that the bonding strength was increased by containing Sn, Ag, and Ir.

  Furthermore, it was excellent in addition to the improvement of joining strength by making content of Ag into 1.5 mass% or more from the airtight test result of Example 1, Example 2, and Example 3-Example 25. It was confirmed that airtightness was exhibited.

  Further, when the oxygen content in the bonding composition was evaluated for Example 25, it was confirmed that the oxygen content was 0.0009 mass% and the oxygen content was 0.0001 mass% or more. Further, it was confirmed that the bonding strength was sufficiently higher than those of Comparative Examples 1 to 5.

Claims (7)

Contains tin, silver, and iridium,
Containing tin as a main component,
A bonding composition containing 0.5% by mass or more and 11.0% by mass or less of the silver.   The bonding composition according to claim 1, comprising 0.001% by mass or more and 1.0% by mass or less of the iridium.   Furthermore, the composition for joining of Claim 1 or 2 containing 0.001 mass% or more and 0.8 mass% or less of aluminum.   Further, germanium is 0% by mass to 1.0% by mass, nickel is 0% by mass to 1.0% by mass, copper is 0% by mass to 0.1% by mass, and magnesium is 0% by mass to 0.5% by mass. The bonding composition according to any one of claims 1 to 3, which is contained.   The bonding composition according to any one of claims 1 to 4, wherein the oxygen content is 0.0001 mass% or more and 2 mass% or less.   The bonding composition according to any one of claims 1 to 5, which is used when a material to be bonded containing an oxide is bonded to a bonding portion.   The bonding composition according to claim 6, wherein the oxide is at least one selected from glass, chromium oxide, and aluminum oxide.

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